A high-efficient stable surface-prelithiated Li1.2Ni0.13Co0.13Mn0.54O2 cathode enabled by sacrificial lithium nitrides for high-energy-density lithium-ion batteries

Lithium-rich cathode materials with superior practical specific capacity over 250 mAh g−1 are considered as one of the resolutions for high-energy-density lithium-ion batteries, while the intrinsic capacity loss caused by solid electrolyte interface (SEI) formation on the anode impedes the increase of energy density. To address this issue, we propose a composite cathode prelithiation strategy including a carbon-incorporated lithium phosphorus oxynitride (LiCPON) layer and a sacrificial Li3N (Sac. Li3N) layer, which can not only compensate for the capacity loss effectively and controllably with a high lithium utilization rate over 85% but also provide outstanding atmosphere stability with an 80.2% lithium utilization rate after exposed in dry air for 8 hours. The energy densities achieve 489.5 Wh kg−1 and 497.3 Wh kg−1 initially after cathode prelithiation in full cells paired with Si/C and SiOx/C anodes, corresponding to a 11.9% and 11.6% increase, respectively. The energy densities still remain 318.7 Wh kg−1 and 319.7 Wh kg−1 after 50 cycles with an increase of 13.7% and 11.7%, respectively. The cathode electrolyte interface (CEI) and SEI layers are mutually optimized and the electrolyte adsorption and degradation are suppressed after cathode prelithiation. Our work has demonstrated that such a composite cathode prelithiation strategy provides the possibility for large-scale industrial production, transportation, and conservation of prelithiated lithium-rich cathodes to achieve high-energy-density lithium-ion batteries.